苯甲醇氧化制苯甲酸钠反应中金钯双金属催化剂的协同效应

doi:10.1016/S1872-2067(14)60159-5

催化学报 ›› 2014, Vol. 35 ›› Issue (11): 1846-1857.DOI: 10.1016/S1872-2067(14)60159-5

苯甲醇氧化制苯甲酸钠反应中金钯双金属催化剂的协同效应

张召艳, 王英, 李娴, 戴维林

复旦大学化学系, 上海市分子催化和功能材料重点实验室, 上海200433

收稿日期:2014-05-06 修回日期:2014-05-26 出版日期:2014-11-06 发布日期:2014-11-06
通讯作者: 戴维林
基金资助:
国家重点基础研究发展计划(973计划,2012CB224804); 国家自然科学基金(21373054,21173052); 上海市科学技术委员会上海市自然科学基金(08DZ2270500).

Synergistic effect on Au-Pd bimetallic catalyst during oxidation of benzyl alcohol to sodium benzoate

Zhaoyan Zhang, Ying Wang, Xian Li, Wei-Lin Dai

Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China

Received:2014-05-06 Revised:2014-05-26 Online:2014-11-06 Published:2014-11-06
Supported by:
This work was supported by the National Basic Research Program of China (973 Program, 2012CB224804), the National Natural Science Foundation of China (21373054, 21173052), and the Natural Science Foundation of Shanghai Science and Technology Committee (08DZ2270500).

摘要/Abstract

摘要：

研究了不同Au/Pd摩尔比的AuPd/CeO₂双金属催化剂在苯甲醇氧化制苯甲酸及其钠盐反应中的催化活性, 利用XRD, UV-Vis DRS, TEM和XPS等手段对催化剂的结构进行了系统考察. 结果表明, Au-Pd纳米颗粒以合金形式分散在CeO₂载体上, 不同Au/Pd摩尔比会影响催化剂表面活性物种的粒径大小和尺寸分布, 并改变催化剂表面物种的组成. Au-Pd之间的电子效应和协同效应显著影响其催化活性. 当Au/Pd摩尔比为3时催化剂表现出最好的催化活性, 苯甲酸产率可达92%. 此外, 双金属催化剂的催化活性显著优于单金属催化剂, 主要归因于Au和Pd之间的协同效应. AuPd/CeO₂催化剂还具有良好的稳定性, Au/Pd摩尔比为3的AuPd/CeO₂催化剂使用7次后仍然具有较高的催化活性.

关键词: 金, 钯, 氧化铈, 双金属催化剂, 苯甲醇, 催化氧化, 苯甲酸盐

Abstract:

A series of AuPd/CeO₂ bimetallic catalysts with different Au/Pd molar ratios were investigated and their catalytic performance in the oxidation of benzyl alcohol to sodium benzoate and benzoic acid under solvent-free conditions was studied. The supported catalysts were characterized by X-ray diffraction, UV-Vis diffuse reflectance spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. The Au-Pd nanoparticles were successfully deposited onto CeO₂ as a homogeneous alloy. The activity of the bimetallic catalysts was superior to that of the corresponding monometallic catalysts. This improvement was attributed to the synergistic effect between Au and Pd. The catalyst with an Au/Pd molar ratio of 3/1 showed the best catalytic performance (the yield of benzoic acid reached 92%), and it could be easily recovered and reused for more than seven successive reactions without significant loss of activity.

Key words: Gold, Palladium, Ceria, Bimetallic catalyst, Benzyl alcohol, Catalytic oxidation, Benzoate

张召艳, 王英, 李娴, 戴维林. 苯甲醇氧化制苯甲酸钠反应中金钯双金属催化剂的协同效应[J]. 催化学报, 2014, 35(11): 1846-1857.

Zhaoyan Zhang, Ying Wang, Xian Li, Wei-Lin Dai. Synergistic effect on Au-Pd bimetallic catalyst during oxidation of benzyl alcohol to sodium benzoate[J]. Chinese Journal of Catalysis, 2014, 35(11): 1846-1857.

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苯甲醇氧化制苯甲酸钠反应中金钯双金属催化剂的协同效应

Synergistic effect on Au-Pd bimetallic catalyst during oxidation of benzyl alcohol to sodium benzoate

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